Research articles

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  • Electroreduction of CO2 competes with the hydrogen evolution reaction; thus, controlling water’s activity to exclusively act as a proton donor is a desirable yet challenging goal. Now the behaviour of water in aprotic solvents is shown to depend on the solvent’s donor ability, which can modulate the hydrogen bond network and in turn promote the desired reactivity.

    • Reginaldo J. Gomes
    • Ritesh Kumar
    • Chibueze V. Amanchukwu
  • Pt is the most active catalyst for the hydrogen evolution reaction in acidic media, but the precise nature of its active sites remains elusive. Now electrical transport spectroscopy and molecular dynamics are combined to map the hydrogen adsorption sites on Pt nanowires and reveal the much higher activity of (111)/(100) edge sites.

    • Zhihong Huang
    • Tao Cheng
    • Xiangfeng Duan
  • Olefin hydroformylation is traditionally performed with homogeneous catalysts. Here the authors introduce a heterogeneous system based on zeolite-confined Rh clusters that is characterized by high efficiency for the hydroformylation of C6–C12 terminal olefins into linear aldehydes with high selectivity.

    • Xiaomeng Dou
    • Tao Yan
    • Lichen Liu
  • Photoredox-catalysed coupling of electron-rich aryl electrophiles based on simple nickel salts usually suffers from a slow oxidative addition. Now, it is shown that thianthrenation leads to more favourable redox properties of the substrates, alleviating this problem in carbon–heteroatom bond-forming reactions.

    • Shengyang Ni
    • Riya Halder
    • Tobias Ritter
    ArticleOpen Access
  • Direct stereoselective amination of tertiary C–H bonds without the assistance of directing groups is a challenging task in synthetic organic chemistry. Now a nitrene transferase is engineered to aminate tertiary C–H bonds with high enantioselectivity, providing direct access to valuable chiral α-tertiary primary amines.

    • Runze Mao
    • Shilong Gao
    • Frances H. Arnold
  • Asymmetric versions of radical-mediated alkene difunctionalizations featuring hydrocarbon precursors are currently elusive. Here the authors report an asymmetric vicinal alkene dicarbofunctionalization based on the activation of C(sp3)–H bonds through the combination of photocatalysed hydrogen atom transfer and nickel catalysis.

    • Xia Hu
    • Iván Cheng-Sánchez
    • Cristina Nevado
    ArticleOpen Access
  • Synthetic methylotrophic organisms provide potential for valorization of greenhouse gas-derived methanol. Here an Escherichia coli strain is generated that reaches a similar growth rate on methanol to many natural methylotrophs and is capable of producing chemicals from this carbon source.

    • Michael A. Reiter
    • Timothy Bradley
    • Julia A. Vorholt
    ArticleOpen Access
  • The tunable design of molecular catalysts presents opportunities for the control of product selectivity in CO2 reduction, yet to date, complexes capable of producing multicarbon products have been elusive. Here, a Br-bridged dinuclear Cu(I) complex that turns over C3H7OH is reported.

    • Naonari Sakamoto
    • Keita Sekizawa
    • Takeshi Morikawa
    ArticleOpen Access
  • The development of superior and cost-effective catalysts for the oxygen reduction and evolution reactions is pivotal for the future hydrogen economy. Now a series of Ru-modified Li2MnO3 catalysts have been designed to optimize the electronic structure and achieve a high performance in both oxygen reduction and evolution reactions, as demonstrated in practical anion exchange membrane fuel cell and water electrolyser tests.

    • Xuepeng Zhong
    • Lijun Sui
    • Jiwei Ma
  • Photoelectrocatalysis offers the potential to reduce energy demand and provide different selectivity profiles compared with electrocatalytic analogues, but current systems have shown limited rates. Here, recent advances in light concentration and gas diffusion electrodes are integrated into a photoelectrochemical system for coupled glycerol oxidation and CO2/H2O reduction with photocurrent densities above 100 mA cm−2.

    • Ádám Balog
    • Egon Kecsenovity
    • Csaba Janáky
    ArticleOpen Access
  • Oxide-derived copper is well-known as a CO2 reduction electrocatalyst, yet the mechanism of its formation and the structure of the active phase remain unclear. Here the reduction of oxide-derived copper is modelled using large-scale molecular dynamics with a neural network potential, providing important insights into the removal of trapped oxygen under operating conditions.

    • Zan Lian
    • Federico Dattila
    • Núria López
    ArticleOpen Access
  • Photoelectrocatalytic nitrate reduction offers an opportunity for a lower carbon route to ammonia production but has not been realized due to poor efficiency. Here an efficient modified lead halide perovskite photocathode is coupled to glycerol oxidation anode resulting in a bias-free photocurrent density greater than 20 mA cm−2.

    • Ahmad Tayyebi
    • Rashmi Mehrotra
    • Ji-Wook Jang
  • Polar and steric effects usually dictate the regioselectivity in homolytic aromatic substitution. Now a method for direct ortho-selective C–H amination of aromatics with diverse side chains as directing groups is disclosed, by which the iron catalyst coordinates both the substrate and the aminyl radical.

    • Chao-Rui Ma
    • Guan-Wang Huang
    • Fei Wang
  • The semihydrogenation of acetylene is an important industrial reaction generally targeted with alloy catalysts and more recently with single-atom catalysts. Here, the authors report a MOF-supported Pd1–Au1 dimeric system that, by merging such approaches, results in high performance levels under simulated front-end industrial conditions.

    • Jordi Ballesteros-Soberanas
    • Nuria Martín
    • Antonio Leyva-Pérez
    ArticleOpen Access
  • Ethylene oxide is a key platform chemical that is produced industrially from the epoxidation of ethylene on silver catalysts, but the precise mechanism remains elusive. Now, in a joint computational–experimental effort, a phase of the silver catalyst grown on (100) facets that contains square-pyramidal subsurface oxygens and is stabilized by strongly adsorbed ethylene is identified as the active phase, and the mechanism is revealed.

    • Dongxiao Chen
    • Lin Chen
    • Zhi-Pan Liu
  • Nanoparticles are often stabilized by capping ligands but the specific role of such ligands during catalytic processes is often ignored. Now, in situ techniques including spatially resolved infrared nanospectroscopy reveal the ligand-assisted formation of a catalytic microenvironment on the surface of silver nanoparticles with nanoscale precision during CO2 electroreduction.

    • Yu Shan
    • Xiao Zhao
    • Peidong Yang
  • Unstrained aryl–aryl bonds are among the most inert bonds in organic chemistry. Now the development of a split cross-coupling strategy enables the direct functionalization of such bonds through Rh-catalysed C–C cleavage and cross-coupling with aryl halides, providing a method for biaryl synthesis.

    • Congjun Yu
    • Zining Zhang
    • Guangbin Dong
  • The synthesis of well-defined heterostructure interfaces can be leveraged to design advanced catalysts. Now a catalyst consisting of carbon-supported Janus particles with crystalline Ru and amorphous CrOx sides is shown to achieve high performance for both alkaline hydrogen oxidation and evolution reactions due to the synergy between both sides.

    • Bingxing Zhang
    • Jianmei Wang
    • Wenping Sun